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A comparative study demonstrates strong size tunability of carrier-phonon coupling in CdSe-based 2D and 0D nanocrystals

(2019) NANOSCALE. 11(9). p.3958-3967
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Abstract
In a comparative study we investigate the carrier-phonon coupling in CdSe based core-only and hetero 2D as well as 0D nanoparticles. We demonstrate that the coupling can be strongly tuned by the lateral size of nanoplatelets, while, due to the weak lateral confinement, the transition energies are only altered by tens of meV. Our analysis shows that an increase in the lateral platelet area results in a strong decrease in the phonon coupling to acoustic modes due to deformation potential interaction, yielding an exciton deformation potential of 3.0 eV in line with theory. In contrast, coupling to optical modes tends to increase with the platelet area. This cannot be explained by Frohlich interaction, which is generally dominant in II-VI materials. We compare CdSe/CdS nanoplatelets with their equivalent, spherical CdSe/CdS nanoparticles. Universally, in both systems the introduction of a CdS shell is shown to result in an increase of the average phonon coupling, mainly related to an increase of the coupling to acoustic modes, while the coupling to optical modes is reduced with increasing CdS layer thickness. The demonstrated size and CdS overgrowth tunability has strong implications for applications like tuning carrier cooling and carrier multiplication - relevant for solar energy harvesting applications. Other implications range from transport in nanosystems e.g. for field effect transistors or dephasing control. Our results open up a new toolbox for the design of photonic materials.
Keywords
TEMPERATURE-DEPENDENCE, COLLOIDAL NANOPLATELETS, RECOMBINATION DYNAMICS, 2-PHOTON ABSORPTION, FINE-STRUCTURE, QUANTUM DOTS, EMISSION, ELECTRON, SPECTROSCOPY, LINEWIDTH

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MLA
Scott, Riccardo et al. “A Comparative Study Demonstrates Strong Size Tunability of Carrier-phonon Coupling in CdSe-based 2D and 0D Nanocrystals.” NANOSCALE 11.9 (2019): 3958–3967. Print.
APA
Scott, R., Prudnikau, A. V., Antanovich, A., Christodoulou, S., Riedl, T., Bertrand, G. H., Owschimikow, N., et al. (2019). A comparative study demonstrates strong size tunability of carrier-phonon coupling in CdSe-based 2D and 0D nanocrystals. NANOSCALE, 11(9), 3958–3967.
Chicago author-date
Scott, Riccardo, Anatol V Prudnikau, Artsiom Antanovich, Sotirios Christodoulou, Thomas Riedl, Guillaume HV Bertrand, Nina Owschimikow, et al. 2019. “A Comparative Study Demonstrates Strong Size Tunability of Carrier-phonon Coupling in CdSe-based 2D and 0D Nanocrystals.” Nanoscale 11 (9): 3958–3967.
Chicago author-date (all authors)
Scott, Riccardo, Anatol V Prudnikau, Artsiom Antanovich, Sotirios Christodoulou, Thomas Riedl, Guillaume HV Bertrand, Nina Owschimikow, Jörg KN Lindner, Zeger Hens, Iwan Moreels, Mikhail Artemyev, Ulrike Woggon, and Alexander W Achtstein. 2019. “A Comparative Study Demonstrates Strong Size Tunability of Carrier-phonon Coupling in CdSe-based 2D and 0D Nanocrystals.” Nanoscale 11 (9): 3958–3967.
Vancouver
1.
Scott R, Prudnikau AV, Antanovich A, Christodoulou S, Riedl T, Bertrand GH, et al. A comparative study demonstrates strong size tunability of carrier-phonon coupling in CdSe-based 2D and 0D nanocrystals. NANOSCALE. 2019;11(9):3958–67.
IEEE
[1]
R. Scott et al., “A comparative study demonstrates strong size tunability of carrier-phonon coupling in CdSe-based 2D and 0D nanocrystals,” NANOSCALE, vol. 11, no. 9, pp. 3958–3967, 2019.
@article{8607665,
  abstract     = {In a comparative study we investigate the carrier-phonon coupling in CdSe based core-only and hetero 2D as well as 0D nanoparticles. We demonstrate that the coupling can be strongly tuned by the lateral size of nanoplatelets, while, due to the weak lateral confinement, the transition energies are only altered by tens of meV. Our analysis shows that an increase in the lateral platelet area results in a strong decrease in the phonon coupling to acoustic modes due to deformation potential interaction, yielding an exciton deformation potential of 3.0 eV in line with theory. In contrast, coupling to optical modes tends to increase with the platelet area. This cannot be explained by Frohlich interaction, which is generally dominant in II-VI materials. We compare CdSe/CdS nanoplatelets with their equivalent, spherical CdSe/CdS nanoparticles. Universally, in both systems the introduction of a CdS shell is shown to result in an increase of the average phonon coupling, mainly related to an increase of the coupling to acoustic modes, while the coupling to optical modes is reduced with increasing CdS layer thickness. The demonstrated size and CdS overgrowth tunability has strong implications for applications like tuning carrier cooling and carrier multiplication - relevant for solar energy harvesting applications. Other implications range from transport in nanosystems e.g. for field effect transistors or dephasing control. Our results open up a new toolbox for the design of photonic materials.},
  author       = {Scott, Riccardo and Prudnikau, Anatol V and Antanovich, Artsiom and Christodoulou, Sotirios and Riedl, Thomas and Bertrand, Guillaume HV and Owschimikow, Nina and Lindner, Jörg KN and Hens, Zeger and Moreels, Iwan and Artemyev, Mikhail and Woggon, Ulrike and Achtstein, Alexander W},
  issn         = {2040-3364},
  journal      = {NANOSCALE},
  keywords     = {TEMPERATURE-DEPENDENCE,COLLOIDAL NANOPLATELETS,RECOMBINATION DYNAMICS,2-PHOTON ABSORPTION,FINE-STRUCTURE,QUANTUM DOTS,EMISSION,ELECTRON,SPECTROSCOPY,LINEWIDTH},
  language     = {eng},
  number       = {9},
  pages        = {3958--3967},
  title        = {A comparative study demonstrates strong size tunability of carrier-phonon coupling in CdSe-based 2D and 0D nanocrystals},
  url          = {http://dx.doi.org/10.1039/c8nr09458f},
  volume       = {11},
  year         = {2019},
}

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